Exploring the potential of fulvalene dimetals as platforms for molecular solar thermal energy storage: computations, syntheses, structures, kinetics, and catalysis

Chemistry. 2014 Nov 17;20(47):15587-604. doi: 10.1002/chem.201404170. Epub 2014 Oct 3.

Abstract

A study of the scope and limitations of varying the ligand framework around the dinuclear core of FvRu2 in its function as a molecular solar thermal energy storage framework is presented. It includes DFT calculations probing the effect of substituents, other metals, and CO exchange for other ligands on ΔHstorage . Experimentally, the system is shown to be robust in as much as it tolerates a number of variations, except for the identity of the metal and certain substitution patterns. Failures include 1,1',3,3'-tetra-tert-butyl (4), 1,2,2',3'-tetraphenyl (9), diiron (28), diosmium (24), mixed iron-ruthenium (27), dimolybdenum (29), and ditungsten (30) derivatives. An extensive screen of potential catalysts for the thermal reversal identified AgNO3 -SiO2 as a good candidate, although catalyst decomposition remains a challenge.

Keywords: ab initio calculations; iron; isomerization; photochemistry; ruthenium.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Alkadienes / chemistry*
  • Catalysis
  • Coordination Complexes / chemical synthesis*
  • Coordination Complexes / chemistry
  • Crystallography, X-Ray
  • Cyclopentanes / chemistry*
  • Kinetics
  • Metals / chemistry*
  • Molecular Conformation
  • Solar Energy*
  • Thermodynamics

Substances

  • Alkadienes
  • Coordination Complexes
  • Cyclopentanes
  • Metals
  • fulvenallene